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姓名	鄭博駿(Po-Chun Cheng)  查詢紙本館藏	畢業系所	能源工程研究所
論文名稱	提升質子陶瓷燃料電池性能之研究 (Study on Performance Enhancement of Protonic Ceramic Fuel Cell (PCFC))
相關論文	★ 定開孔率下流道設計與疏水流場對質子交換膜燃料電池之性能影響 ★ 熱風循環烘箱熱傳特性研究 ★ 以陽極處理製備奈米結構之氧化鐵光觸媒薄膜應用在光電化學產氫 ★ 規則多孔碳應用在燃料電池陰極觸媒擔體之研究 ★ 鉑錫/多孔碳觸媒應用於燃料電池陰極反應之研究 ★ 腐蝕特性對金屬多孔材質子交換膜燃料電池性能影響之研究 ★ 碎形理論應用在質子交換膜燃料電池中氣體擴散層熱傳導係數之研究 ★ 中溫固態氧化物燃料電池複合系統分析 ★ 中文質子傳輸型固態氧化物燃料電池陽極之研究 ★ 鋯摻雜鋇鈰釔氧化物微結構與電化學特性之研究 ★ 發展應用脈衝雷射沉積製備奈米顆粒堆疊多孔觸媒層與滴塗聚苯並咪唑介面層製作高溫型質子交換膜燃料電池 ★ 直接甲醇燃料電池氣體擴散層之研究 ★ 不同流道設計之透明質子交換膜燃料電池陰極水生成現象探討 ★ 鋰離子電池陰極材料LiCoO2粉體尺寸與形貌對電池性能的影響 ★ 多孔性碳材應用於質子交換膜燃料電池觸媒層之研究 ★ 多孔材應用於質子交換膜燃料電池散熱之研究
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摘要(中)	本研究第一部份旨在為甲烷燃料質子陶瓷燃料電池（PCFC）開發一種比傳統 Ni-BCZY 陽極更好的耐碳陽極。採用固相反應製程製備PCFC中Ni1-xCux-BCZY合金陽極。Ni中摻雜Cu，並在甲烷及氫氣下對陽極支撐型之單電池進行了性能曲線及電化學阻抗頻譜的量測與分析，結果得知當通入氫氣及甲烷時Ni0.9Cu0.1電池皆表現出最佳之電池性能，最高功率密度分別達到409.5 mW/cm2及177.6 mW/cm2，有此可知參雜少量的銅能夠不影響通入甲烷時之電池性能，而參雜的銅過多則使電池性能降低。這項工作證明了採用 Ni1-xCux -BCZY 合金陽極於甲烷燃料之可用性，有助於開發以甲烷做為燃料用於固體氧化物燃料電池發電之合金陽極。 本研究第二部份為了獲得緻密、高品質的電解質，質子陶瓷燃料電池（PCFC）中的質子傳導電解質BaCe0.6Zr0.2Y0.2O3 (BCZY)的燒結應在相對較高的溫度下進行。然而，在多孔陽極基底和電解質薄膜共燒結時，高燒結溫度往往會導致NiO-BCZY陽極粗化，從而減少H2氧化的電催化活性位點數量。 以及降低電池性能。提出了一種可擴展的奈米球磨製程來降低電解質燒結溫度，以維持 PCFC 陽極中的三相邊界、良好的電子和質子傳輸。透過使用奈米球磨製程，生產出的BCZY奈米粒子的直徑減少了一半以上（從 297 nm 到 131 nm）。可以降低共燒結溫度。在1400 ℃下燒結的電池表現出最高功率密度490 mW/cm2，比非奈米製程高38%。電池性能的顯著改善可歸因於較低的共燒結溫度，從而減少了 NiO 陽極的粗化。這保留了更多數量的H2電催化活性位點 電化學阻抗測量顯示電荷轉移電阻降低了 50%，證明了電池運作中 Ni 的氧化作用。 進一步將奈米粉末應用於陽極功能層，將球磨4小時之奈米粉末(135.4 nm)運用於固態氧化物燃料電池之陽極功能層，製備不同奈米AFL層分別為一層奈米AFL、二層奈米AFL及原始和奈米結合之複合AFL，其功率密度分別為286.1 mW/cm2、463.3 mW/cm2及534.1 mW/cm2，可以發現原始和奈米結合之複合AFL其電池性能有明顯提升相較於原始陽極功能層時其功率密度增加9%。進一步透過EIS分析可以看到複合AFL其活化極化RPh有明顯的下降趨勢，由於奈米AFL平均顆粒直徑減少一半，進而增加更多的三相介面導致活化極化降低。由結果得知本研究將奈米製程應用於AFL可以有效增加與電解質間的界面接觸進而降低歐姆阻抗及極化阻抗，進一步提升電池性能。 本研究第三部份提出一種能夠改善電解質多孔界面層與電解質之間接觸界面的新方法，透過共燒結多孔界面層與電解質之方法可以達到較好的接觸界面，降低電池內的界面阻抗進而實現更高的功率密度。研究結果顯示，共燒結之電解質多孔界面層電池於800 ℃下測得最大功率密度為429.3 mW/cm2，相較於預燒結之電解質多孔界面層電池(336.4 mW/cm2)其電池最大功率密度提升了17.2%，歐姆阻抗降低約30.8%。由結果得知透過共燒結多孔界面層與電解質之方法可以達到較好的接觸界面降低阻抗，進一步改善PCFC之電池性能。
摘要(英)	The first part of this study aimed to develop a carbon-resistant anode for methane-fueled protonic ceramic fuel cells (PCFC) that is better than the conventional Ni-BCZY anode. The Ni1-xCux-BCZY alloy in the PCFC anode was prepared using a solid-state reaction process. Ni is doped with Cu to the anode-supported single cell′s performance curve and electrochemical impedance spectrum were measured and analyzed under methane and hydrogen. The results showed that the Ni0.9Cu0.1 cell performed best when introduced to hydrogen and methane. Regarding cell performance, the highest power density reached 409.5 mW/cm2 and 177.6 mW/cm2, respectively. Results show that doping a small amount of cobalt will not affect the cell performance when introducing methane. On the other hand, doping too much copper will reduce cell performance. This work demonstrates the usability of the Ni1-xCux-BCZY alloy anode for methane fuel, and helps to develop alloy anodes for solid oxide fuel cell power generation using methane. The second part of this study aims to obtain a dense, high-quality electrolyte. The proton conducting electrolyte BaCe0.6Zr0.2Y0.2O3 (BCZY) sintering for the protonic ceramic fuel cell (PCFC) was carried out at a relatively high temperature. However, when the porous anode substrate and the electrolyte film are co-sintered, the high sintering temperature often leads to the coarsening of the NiO-BCZY anode, thereby reducing the number of electro-catalytic active sites for H2 oxidation and reduced cell performance. A scalable nanoball milling process is proposed to reduce the electrolyte sintering temperature to maintain a three-phase boundary and enhance electron and proton transport in PCFC anodes. Using the nanoball milling process, the BCZY nanoparticles′ diameter was reduced by more than half (from 297 nm to 131 nm). The co-sintering temperature can be lowered. The cell sintered at 1400 °C showed the highest peak power density of 490 mW/cm2, 38% higher than the non-nano-milling process. The significant improvement in cell performance can be attributed to the lower co-sintering temperature, which reduces the coarsening of the NiO anode. This preserves a more substantial number of H2 electrocatalytically active sites. Electrochemical impedance measurements show a 50% reduction in charge transfer resistance, demonstrating the oxidation of Ni in cell operation. The nano-powder was further applied to the anode functional layer. The nano-powder (135.4 nm) was ball-milled for 4 hours and applied to the anode functional layer of the solid oxide fuel cell to prepare different nano AFL layers, including one layer of nano AFL and two layers of nano AFL. The power densities of the layered nano-AFL, the original, and nano-combined composite AFL are 286.1 mW/cm2, 463.3 mW/cm2, and 534.1 mW/cm2, respectively. It can be found that the cell performance of the original and nano-combined composite AFL has been significantly improved. Compared with the original anode functional layer, its power density increases by 9%. Further EIS analysis shows that the activation polarization RPh of composite AFL has a clear downward trend. Since the average particle diameter of nano-AFL is reduced by half, more three-phase interfaces are added, decreasing activation polarization. It is known from the results that the application of the nanometer manufacturing process to AFL in this study can effectively increase the interface contact with the electrolyte, reduce ohmic impedance and polarization resistance, and further improve cell performance. The third part of this study proposes a new method that can improve the contact interface between the porous interface layer and the electrolyte. By co-sintering the porous interface layer and the electrolyte, a better contact interface can be achieved, and the interface impedance in the cell can be reduced. This results in higher power density. This research results show that the maximum power density of the co-sintered electrolyte porous interface layer cell measured at 800°C is 429.3 mW/cm2. Compared with the pre-sintered electrolyte porous interface layer cell (336.4 mW/cm2), the maximum power density of the cell is improved by 17.2%, and the ohmic impedance is reduced by about 30.8%. The results show that by co-sintering the porous interface layer and the electrolyte, a better contact interface can be achieved to reduce the impedance and further improve the cell performance of PCFC.
關鍵字(中)	★ 質子陶瓷燃料電池 ★ 鎳銅合金 ★ 甲烷 ★ 奈米球磨 ★ 共燒結溫度 ★ 陽極粗化 ★ 複合陽極功能層 ★ 多孔層	關鍵字(英)	★ Protonic ceramic fuel cells ★ NiCu alloy ★ Methane ★ Nanomilling ★ Co-sintering temperature ★ Anode coarsening ★ Composite anode functional layer ★ Porous layers
論文目次	碩博士論文電子檔授權書 II 延後公開申請書 III 論文指導教授推薦書 IV 論文口試委員審定書 V 摘要 VI Abstract VIII 致謝 XI 目錄 XII 圖目錄 XVI 表目錄 XXI 第一章、緒論 1 1-1 前言 1 1-2 燃料電池 3 1-3 固態氧化物燃料電池 4 1-3-1 P-SOFC及O-SOFC原理 4 1-4 PCFC材料之特性 6 1-4-1 PCFC陽極材料 9 1-4-2 PCFC電解質材料 11 1-4-3 PCFC陰極材料 13 1-5 粉末合成方法與燒結機制 15 1-5-1 粉末合成方法 15 1-5-2 粉末燒結理論 16 1-6 P-SOFC電池製備技術 18 1-6-1 刮刀成型技術(Tape casting methode) 18 1-6-2 乾壓成型技術(Dry pressing methode) 19 1-6-3 旋轉塗布技術(Spin coating methode) 19 1-6-4 絲網印刷技術(Screen printing methode) 20 1-7 研究目的 21 第二章、文獻回顧 23 2-1 甲烷對SOFC之影響 23 2-1-1 改變NiCu合金比例對陽極材料性質的影響 23 2-2 固態反應法製備高品質奈米粉末 25 2-2-1 低缺陷電解質層對SOFC之影響 26 2-2-2 燒結溫度對SOFC之影響 28 第三章、實驗方法 29 3-1 實驗藥品 29 3-2 實驗製程設備 30 3-3 實驗流程與方法 32 3-3-1 電解質粉末製備 32 3-3-2 陽極支撐型之基板製備 33 3-3-3 NiCu陽極粉末製備 34 3-3-4 奈米電解質漿料製備 35 3-3-5 奈米陽極功能層漿料製備 36 3-3-6 電解質多孔界面層製備 37 3-3-7 單電池製備 38 3-4 電池分析儀器 39 3-4-1 X光繞射儀(X-Ray Diffraction, XRD) 39 3-4-2 掃描式電子顯微鏡(Scanning Electron Microscope, SEM) 40 3-4-3 導電度阻抗儀(Conductivity measurement) 41 3-4-4 雙束型聚焦離子束(Dual-beam focused ion beam, DB-FIB) 42 3-4-5 雷射粒徑分析儀(DLS Nano particle size analyzer) 43 3-4-6 燃料電池I-V性能量測與分析 43 3-4-7 電化學交流阻抗量測與分析 46 第四章、結果與討論 48 4-1 Ni1-xCux-BCZY合金陽極於甲烷燃料之電池性能 48 4-1-1 Ni1-xCux-BCZY 陽極材料分析 48 4-1-2 Ni1-xCux-BCZY合金陽極電池性能分析 49 4-1-3 Ni1-xCux-BCZY合金陽極 - 小結 54 4-2 奈米球磨製程製備奈米級粉末 55 4-2-1 奈米粉末分析 55 4-2-2 奈米薄膜 61 4-2-3 微結構分析 63 4-2-4 奈米球磨製程製備奈米級粉末 - 小結 67 4-3 奈米電解質層降低PCFC共燒結溫度 67 4-3-1 奈米電解質層 67 4-3-2 電池性能分析 69 4-3-3 PCFC陽極微結構 73 4-3-4 奈米電解質層降低PCFC共燒結溫度 - 小結 76 4-4 奈米粉末應用於陽極功能層 77 4-4-1 I-V性能曲線量測與分析 77 4-4-2 交流阻抗量測與分析 79 4-4-3 微結構分析 80 4-4-4 奈米球磨應用於陽極功能層 - 小結 81 4-5 BCZY電解質多孔界面層 82 4-5-1 材料及形貌分析 82 4-5-2 I-V性能曲線量測與分析 83 4-5-3 交流阻抗量測與分析 84 4-5-4 微結構分析 86 4-5-5 BCZY電解質多孔界面層 - 小結 87 第五章、結論與未來規劃 88 5-1 結論 88 5-2 未來規劃 91 參考文獻 92
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指導教授	曾重仁(Chung-Jen Tseng)	審核日期	2023-10-24
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